Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates

[EN] Heterometallic lanthanide [LnLn'] coordination complexes that are accessible thermodynamically are very scarce because the metals of this series have very similar chemical behaviour. Trinuclear systems of this category have not been reported. A coordination chemistry scaffold has been show...

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Autores: Maniaki, Diamantoula, Garay Ruiz, Diego, Barrios Moreno, Leoní Alejandra, Martins, Daniel O.T. A., Aguilà, David, Tuna, Floriana, Reta Mañeru, Daniel, Roubeau, Olivier, Bo, Carles, Aromí, Guillem
Tipo de recurso: artículo
Fecha de publicación:2022
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/56681
Acceso en línea:http://hdl.handle.net/10810/56681
Access Level:acceso abierto
Palabra clave:lanthanide complexes
energy transfer
luminescence
contraction
Ln (III)
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spelling Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gatesManiaki, DiamantoulaGaray Ruiz, DiegoBarrios Moreno, Leoní AlejandraMartins, Daniel O.T. A.Aguilà, DavidTuna, FlorianaReta Mañeru, DanielRoubeau, OlivierBo, CarlesAromí, Guillemlanthanide complexesenergy transferluminescencecontractionLn (III)[EN] Heterometallic lanthanide [LnLn'] coordination complexes that are accessible thermodynamically are very scarce because the metals of this series have very similar chemical behaviour. Trinuclear systems of this category have not been reported. A coordination chemistry scaffold has been shown to produce molecules of type [LnLn'Ln] of high purity, i.e. exhibiting high metal distribution ability, based on their differences in ionic radius. Through a detailed analysis of density functional theory (DFT) based calculations, we discern the energy contributions that lead to the unparalleled chemical selectivity of this molecular system. Some of the previously reported examples are compared here with the newly prepared member of this exotic list, [Er2Pr(LA)(2)(LB)(2)(py)(H2O)(2)](NO3) (1) (H(2)LA and H2LB are two beta-diketone ligands). A magnetic analysis extracted from magnetization and calorimetry determinations identifies the necessary attributes for it to act as an addressable, conditional multiqubit spin-based quantum gate. Complementary ab initio calculations confirm the feasibility of these complexes as composite quantum gates, since they present well-isolated ground states with highly anisotropic and distinct g-tensors. The electronic structure of 1 has also been analyzed by EPR. Pulsed experiments have allowed the establishment of the quantum coherence of the transitions within the relevant spin states, as well as the feasibility of a coherent control of these states via nutation experiments.The authors thank the European Union's Horizon 2020 research and innovation programmes QUANTERA project SUMO and FET-OPEN grant 862893 FATMOLS (GA and OR) the Spanish AEI for grants PGC2018-098630-B-I00 (GA and DA), PID2020-118329RB-I00 (OR), PID2020-112806RB-I00 (DGR and CB) and the Severo Ochoa Excellence Accreditation 2020-2023 CEX2019-000925-S (DGR and CB), the ICIQ foundation (DGR and CB) and the Generalitat de Catalunya for a Beatriu de Pinos fellowship (2019-BP-00015, DR), an FI grant (also financed by AGAUR and the European Social Fund, DGR) an FI-SDUR Grant (2020-FISDU-00492, DM), the CERCA program and the ICREA Academia 2018 Prize (GA), as well as the National EPR Facility at the University of Manchester for support with the EPR measurements. This work used resources of the ALBA synchrotron through access to beamline 13-XALOC.Royal Society of ChemistryEuropean Commission202220222022info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/56681reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/EC/H2020/862893info:eu-repo/grantAgreement/MICIU/PGC2018-098630-B-I00/info:eu-repo/grantAgreement/MICINN/PID2020-118329RB-I00/info:eu-repo/grantAgreement/MICINN/PID2020-112806RB-I00/info:eu-repo/grantAgreement/MICINN/CEX2019-000925-S/https://pubs.rsc.org/en/content/articlelanding/2022/SC/D2SC00436Dinfo:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc/3.0/es/© 2022 The Author(s). Published by the Royal Society of Chemistry. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported (CC BY-NC 3.0) licence.Atribución-NoComercial 3.0 Españaoai:addi.ehu.eus:10810/566812026-06-18T09:23:17Z
dc.title.none.fl_str_mv Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
title Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
spellingShingle Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
Maniaki, Diamantoula
lanthanide complexes
energy transfer
luminescence
contraction
Ln (III)
title_short Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
title_full Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
title_fullStr Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
title_full_unstemmed Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
title_sort Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates
dc.creator.none.fl_str_mv Maniaki, Diamantoula
Garay Ruiz, Diego
Barrios Moreno, Leoní Alejandra
Martins, Daniel O.T. A.
Aguilà, David
Tuna, Floriana
Reta Mañeru, Daniel
Roubeau, Olivier
Bo, Carles
Aromí, Guillem
author Maniaki, Diamantoula
author_facet Maniaki, Diamantoula
Garay Ruiz, Diego
Barrios Moreno, Leoní Alejandra
Martins, Daniel O.T. A.
Aguilà, David
Tuna, Floriana
Reta Mañeru, Daniel
Roubeau, Olivier
Bo, Carles
Aromí, Guillem
author_role author
author2 Garay Ruiz, Diego
Barrios Moreno, Leoní Alejandra
Martins, Daniel O.T. A.
Aguilà, David
Tuna, Floriana
Reta Mañeru, Daniel
Roubeau, Olivier
Bo, Carles
Aromí, Guillem
author2_role author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv European Commission
dc.subject.none.fl_str_mv lanthanide complexes
energy transfer
luminescence
contraction
Ln (III)
topic lanthanide complexes
energy transfer
luminescence
contraction
Ln (III)
description [EN] Heterometallic lanthanide [LnLn'] coordination complexes that are accessible thermodynamically are very scarce because the metals of this series have very similar chemical behaviour. Trinuclear systems of this category have not been reported. A coordination chemistry scaffold has been shown to produce molecules of type [LnLn'Ln] of high purity, i.e. exhibiting high metal distribution ability, based on their differences in ionic radius. Through a detailed analysis of density functional theory (DFT) based calculations, we discern the energy contributions that lead to the unparalleled chemical selectivity of this molecular system. Some of the previously reported examples are compared here with the newly prepared member of this exotic list, [Er2Pr(LA)(2)(LB)(2)(py)(H2O)(2)](NO3) (1) (H(2)LA and H2LB are two beta-diketone ligands). A magnetic analysis extracted from magnetization and calorimetry determinations identifies the necessary attributes for it to act as an addressable, conditional multiqubit spin-based quantum gate. Complementary ab initio calculations confirm the feasibility of these complexes as composite quantum gates, since they present well-isolated ground states with highly anisotropic and distinct g-tensors. The electronic structure of 1 has also been analyzed by EPR. Pulsed experiments have allowed the establishment of the quantum coherence of the transitions within the relevant spin states, as well as the feasibility of a coherent control of these states via nutation experiments.
publishDate 2022
dc.date.none.fl_str_mv 2022
2022
2022
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/56681
url http://hdl.handle.net/10810/56681
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/EC/H2020/862893
info:eu-repo/grantAgreement/MICIU/PGC2018-098630-B-I00/
info:eu-repo/grantAgreement/MICINN/PID2020-118329RB-I00/
info:eu-repo/grantAgreement/MICINN/PID2020-112806RB-I00/
info:eu-repo/grantAgreement/MICINN/CEX2019-000925-S/
https://pubs.rsc.org/en/content/articlelanding/2022/SC/D2SC00436D
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by-nc/3.0/es/
Atribución-NoComercial 3.0 España
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by-nc/3.0/es/
Atribución-NoComercial 3.0 España
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,300724

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